Published June 6, 2023 | Version v1
Journal article Open

Impact of solid-electrolyte interphase reformation on capacity loss in silicon-based lithium-ion batteries

  • 1. Materials Center Leoben Forschung GmbH, A8700 Leoben, Austria
  • 2. WMG, University of Warwick, Coventry CV4 7AL, United Kingdom
  • 3. Carl Zeiss Microscopy GmbH, Oberkochen, Germany
  • 4. Varta Micro Innovation GmbH, A8010 Graz, Austria

Description

High-density silicon composite anodes show large volume changes upon charging/discharging triggering the reformation of the solid electrolyte interface (SEI), an interface initially formed at the silicon surface. The question remains how the reformation process and accompanied material evolution, in particular for industrial up-scalable cells, impacts cell performance. Here, we develop a correlated workflow incorporating X-ray microscopy, field-emission scanning electron microscopy tomography, elemental imaging and deep learning-based microstructure quantification suitable to witness the structural and chemical progression of the silicon and SEI reformation upon cycling. The nanometer-sized SEI layer evolves into a micron-sized silicon electrolyte composite structure at prolonged cycles. Experimental-informed electrochemical modelling endorses an underutilisation of the active material due to the silicon electrolyte composite growth affecting the capacity. A chemo-mechanical model is used to analyse the stability of the SEI/silicon reaction front and to investigate the effects of material properties on the stability that can affect the capacity loss.

Notes

We acknowledge the financial support from the European Union (EU) under the Horizon 2020 research and innovation programme (grant agreement No. 875514 "ECO2LIB" and partly by Die Österreichische Forschungsförderungsgesellschaft (FFG) under Mobilität der Zukunft, Proj. No. 891479 "OpMoSi". We acknowledge support from A. Schneemann for XRM measurements, H. Stegmann for acquiring FIB-ToF-SIMS data and T. Volkenandt for EDS measurements all from Zeiss.

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Funding

ECO2LIB – Ecologically and Economically viable Production and Recycling of Lithium-Ion Batteries 875514
European Commission